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Tri-functional electrocatalysis with mass transfer-optimized 3D NiCo alloy for continuous energy conversion system 三功能电催化与传质优化三维NiCo合金连续能量转换系统。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-02-01 DOI: 10.1016/j.jcis.2026.140024
Gangwen Fu , Yu Tian , Yong Gao , Jingwen Qiu , Yuxuan Wang , Wenbo Zhao , Leiqing Cao , Junyuan He , Mengyang Li , Zhenghui Pan , Yu Lei , Zongkui Kou , Jun Ding , Xi Xu
Mass transfer limitations directly govern the utilization efficiency of active sites in gas-involving reactions, thereby hindering intrinsically active sites from functioning effectively at high current densities. Consequently, designing porous structures to improve the transport efficiency of both reactants and products constitutes a central challenge for realizing efficient and stable electrocatalytic processes. To address this challenge, a nickel‑cobalt (NiCo) alloy was fabricated via digital light processing (DLP) technology, and cobalt-nanocarbon (Co NC) active material was incorporated in situ to establish a robust catalytic system. Furthermore, the deliberate structural design promoted bubble mass-transfer kinetics, thereby further improving its performance across multiple catalytic reactions. The electrolysis water device composed of it can operate stably for over 500 h at a current density of 500 mA cm−2 and a voltage of 1.78 V. The assembled zinc-air battery shows a peak power density of 73.5 mW cm−2 and outstanding cyclic durability, lasting for over 300 h. More importantly, the assembled integrated device generates an equivalent amount of hydrogen during both day and night. This innovative strategy offers a reliable reference for the practical implementation of three-dimensional electrodes in highly efficient mass transfer reactions.
在涉及气体的反应中,传质限制直接决定了活性位点的利用效率,从而阻碍了本质活性位点在高电流密度下有效地发挥作用。因此,设计多孔结构以提高反应物和产物的传输效率是实现高效稳定电催化过程的核心挑战。为了解决这一挑战,研究人员通过数字光处理(DLP)技术制造了镍钴(NiCo)合金,并在原位加入了钴纳米碳(Co NC)活性材料,以建立一个强大的催化系统。此外,精心设计的结构促进了气泡传质动力学,从而进一步提高了其在多种催化反应中的性能。由其组成的电解水装置在电流密度为500 mA cm-2、电压为1.78 V的条件下可稳定工作500 h以上。组装后的锌-空气电池的峰值功率密度为73.5 mW cm-2,循环耐久性突出,持续时间超过300小时。更重要的是,组装后的集成装置在白天和晚上都能产生等量的氢气。这一创新策略为三维电极在高效传质反应中的实际应用提供了可靠的参考。
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引用次数: 0
Propelling lithium transport kinetics and inhibiting Al corrosion by high-coordination-strength anion for low-temperature lithium-metal batteries 高配位强度阴离子促进锂离子输运动力学及抑制低温锂金属电池铝腐蚀
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-02-04 DOI: 10.1016/j.jcis.2026.140051
Jin-Xiu Chen , Fei Zhao , Tong Wu , Jin-Hao Zhang , Xiao-Zhong Fan , Zhi-Yuan Gu , Xiao-Dong Chen , Xin-Bing Cheng , Lin Zhu , Yu-Zhen Zhao , Long Kong
The deployment of high-voltage lithium metal batteries (LMBs) under low-temperature conditions holds considerable importance for the advancement of fast charging technologies. Nevertheless, such deployment necessitates electrolyte designs with contradictory requirements, most notably in the realm of solvation structure. Principally, the lithium salts with weakly coordinated anions facilitate the rapid Li+ transport due to large population of solvent separated ion pairs (SSIPs) and low energy of de-anion process at low temperatures. However, such salts corrode aluminum (Al) foil and worsen the battery stability at high voltages. Herein, this fundamental conflict has been unified through surface electric field and interface compositions. The strongly coordinated anions exhibit higher negative charge density due to its high electron constraining capability, as demonstrated with electron localization function (ELF) and nuclear magnetic resonance (NMR). Such characteristic drives them to exhibit faster migration towards the against direction of Li+ under un electric field and hence facilitate the Li+ de-coordination. Meanwhile, the X-ray photoelectron spectroscopy (XPS) demonstrated that the strongly coordinated anions benefit the formation of Li2CO3 and Li2O in solid electrolyte interface (SEI), which exerts a stronger attraction on the Li+ of solvation structure, thereby assisting the Li+ de-coordination process. The contradiction between Li+ transport kinetics and Al corrosion can be unified with high-coordination-strength anion at low-temperature. This formulated electrolyte enables stable operation of high-voltage LMBs even at low temperatures, demonstrating a practical guiding principle for extreme-condition batteries.
低温条件下高压锂金属电池(lmb)的部署对快速充电技术的发展具有重要意义。然而,这种部署需要电解质设计具有矛盾的要求,特别是在溶剂化结构领域。具有弱配位阴离子的锂盐主要是由于大量的溶剂分离离子对(SSIPs)和低温下低能量的脱阴离子过程促进了Li+的快速迁移。然而,这些盐会腐蚀铝(Al)箔,并降低电池在高压下的稳定性。本文通过表面电场和界面组成统一了这一基本冲突。电子定位函数(ELF)和核磁共振(NMR)表明,强配位阴离子具有较高的电子约束能力,因此具有较高的负电荷密度。这一特性促使它们在非电场条件下向Li+反方向快速迁移,有利于Li+的脱配。同时,x射线光电子能谱(XPS)表明,强配位阴离子有利于固体电解质界面(SEI)中Li2CO3和Li2O的形成,对溶剂化结构中的Li+产生更强的吸引力,从而促进Li+的脱配过程。Li+输运动力学与Al腐蚀之间的矛盾可以用低温下高配位强度阴离子来统一。这种配方的电解质即使在低温下也能使高压lmb稳定运行,为极端条件下的电池提供了实用的指导原则。
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引用次数: 0
Cooperative dual-wavelength energy storage in self-powered perovskite NIR cryptodetectors 自供电钙钛矿近红外密码探测器的协同双波长能量存储
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-01-16 DOI: 10.1016/j.jcis.2026.139921
Xinyao Dong , Jianing Fan , Xingyu Wu , Sen Liu , Yuhan Jing , Ziyi Zhao , Qiyue Tang , Xiumei Yin , Wen Xu , Bin Dong
While optical encryption enhances data security, conventional single-wavelength protocols remain vulnerable to interception due to limited dynamic decryption capabilities. Here, we report a cooperative dual-wavelength (980/1550 nm) energy storage mechanism in Er3+, Tm3+ co-doped Cs2NaYbCl6 nanoparticles, achieving a 53.8-fold enhancement in red emission compared to single-wavelength excitation. Leveraging this synergy, we developed a self-powered photodetector (FTO/PEDOT: PSS/PVP-MAPbI2.5Br0.5/PCBM/Ag) featuring polyvinylpyrrolidone-induced defect states and an optimized halide composition (I/Br = 5:1). This architecture enables wavelength-selective charge trapping, effectively restricting device activation to synchronized dual-wavelength inputs. By integrating time-domain multiplexing with wavelength selective thresholds, we implement AND-gate logic encryption, where 1550 nm radiation encodes the data and 980 nm serves as the decoding key. Compared to traditional single-wavelength systems, this dual-authentication protocol significantly enhances anti-interception capabilities and enables direct optical-domain key verification, eliminating the requirement for complex optoelectronic conversion modules or dedicated processing chips.
虽然光学加密增强了数据安全性,但由于有限的动态解密能力,传统的单波长协议仍然容易被拦截。在这里,我们报道了Er3+, Tm3+共掺杂Cs2NaYbCl6纳米粒子的合作双波长(980/1550 nm)储能机制,与单波长激发相比,实现了53.8倍的红光发射增强。利用这种协同作用,我们开发了一种自供电光电探测器(FTO/PEDOT: PSS/PVP-MAPbI2.5Br0.5/PCBM/Ag),具有聚乙烯吡咯烷酮诱导的缺陷状态和优化的卤化物组成(I-/Br- = 5:1)。该架构支持波长选择性电荷捕获,有效地限制器件激活到同步双波长输入。通过将时域复用与波长选择阈值相结合,我们实现了与门逻辑加密,其中1550 nm的辐射对数据进行编码,980 nm作为解码密钥。与传统的单波长系统相比,这种双认证协议显著增强了抗拦截能力,并实现了直接的光域密钥验证,消除了对复杂光电转换模块或专用处理芯片的需求。
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引用次数: 0
Oppositely directed epitaxial growth of nickel (oxy)hydroxide amorphous oxygen-deficient skin for effective oxygen evolution 用于有效析氧的镍(氧)氢氧化物无定形贫氧皮肤的反向外延生长。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-01-30 DOI: 10.1016/j.jcis.2026.140015
Xiaoqing Cheng , Ze Li , Yuhui Huang , Fanjia Sun , Liang Dong , Youbin Zheng , Jianbing Zang , Jinsheng Li , Ruixia Zhong , Pengfei Li , Zheng-Jun Wang
The amorphous nickel (oxy)hydroxides (NiOx(OH)y) with enriched oxygen vacancies (Ov) grown on the surface of Ni3S2 substrate were designed to boost oxygen evolution reaction (OER) activity. The achieved electrocatalysts showed excellent OER performance with ηj10 of 130 mV, ηj100 of 256 mV, and stability for at least 375 h, outperforming the commercial RuO2 catalysts and most of the state-of-the-art OER catalysts. A new universal stoichiometric mismatch method was developed to synthesize this special structure—by etching low-sulfur-content sulfides in an alkaline aqueous environment to guide the formation of oxygen-deficient amorphous metal oxides. Further, to obtain well-direction low-sulfur nickel sulfide, a novel reverse epitaxial growth method was developed. In this method, in-situ prepared [001]- direction nano Bi2S3 needles were deposited on nickel foam, guiding the substrate to transform into [001]-direction Ni3S2 while causing Bi to detach from the surface. Here, the as-obtained amorphous oxygen-deficient material effectively activates lattice oxygen, and the oxygen vacancies along with the amorphous character at the Ni3S2-NiOx(OH)y interface trigger a unique charge transfer effect, fully activating the surface to promote OER.
设计了在Ni3S2衬底表面生长富氧空位(Ov)的无定形镍(氧)氢氧化物(NiOx(OH)y)以提高析氧反应(OER)活性。所制备的电催化剂表现出优异的OER性能,ηj10为130 mV, ηj100为256 mV,稳定性至少为375 h,优于工业RuO2催化剂和大多数最先进的OER催化剂。提出了一种新的通用化学计量错配方法来合成这种特殊的结构——通过在碱性水环境中蚀刻低硫硫化物来指导贫氧无定形金属氧化物的形成。此外,为了获得井向低硫硫化镍,开发了一种新的反向外延生长方法。该方法将原位制备的[001]向纳米Bi2S3针沉积在泡沫镍上,引导衬底转变为[001]向Ni3S2,同时使Bi与表面分离。在这里,获得的无定形缺氧材料有效地激活了晶格氧,并且在Ni3S2-NiOx(OH)y界面上的氧空位以及无定形特性触发了独特的电荷转移效应,充分激活了表面以促进OER。
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引用次数: 0
Interface-stabilized gel polymer electrolyte for high-performance lithium metal batteries 用于高性能锂金属电池的界面稳定凝胶聚合物电解质。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-02-01 DOI: 10.1016/j.jcis.2026.140029
Chenxi Zhu , Yan Zhao , Rui Xu , Wenqing Lv , Yao Zhao , Bin Huang , Hua-Feng Fei , Zhijie Zhang
Lithium metal batteries demand electrolytes that combine high ionic conductivity with mechanical robustness and interfacial stability. This study presents a novel composite gel polymer electrolyte (GPE) engineered by integrating a cyano-functionalized polysiloxane (PCMS) frameworks, diethylene glycol dimethyl ether (DEGDME) plasticizers, and electrospun polyacrylonitrile (PAN) nanofiber scaffolds. The optimized GPE system achieves an exceptional combination of properties: high ionic conductivity (3.3 × 10−3 S cm−1 at 30 °C), outstanding Li+ transference number (0.79), and remarkable mechanical strength (3.9 MPa). Theoretical calculations and experimental analyses collectively confirm that the -CN groups competitively coordinate with Li+, restructuring the solvation environment to favor TFSI anion participation, thereby facilitating the formation of a robust solid electrolyte interphase (SEI) enriched with LiF and Li₃N. As a result, the GPE demonstrates a wide electrochemical stability window (5.3 V vs. Li+/Li) and stable lithium plating/stripping for 1000 h at 0.1 mA cm−2. Additionally, LiFePO₄/GPE/Li full cells achieve 94.9% capacity retention after 500 cycles at 0.5C, while NCM811/GPE/Li cells deliver a high discharge capacity of 153.8 mAh g−1 with 86.5% retention after 150 cycles. This work establishes a scalable and promising strategy for the development of high-performance lithium metal batteries.
锂金属电池需要结合高离子导电性、机械稳健性和界面稳定性的电解质。本研究提出了一种新型复合凝胶聚合物电解质(GPE),该电解质由氰基功能化聚硅氧烷(PCMS)框架、二甘醇二甲醚(DEGDME)增塑剂和静电纺聚丙烯腈(PAN)纳米纤维支架组成。优化后的GPE体系具有优异的综合性能:高离子电导率(30°C时为3.3 × 10-3 S cm-1)、优异的Li+转移数(0.79)和优异的机械强度(3.9 MPa)。理论计算和实验分析共同证实了- cn基团与Li+竞争性地协调,重组了溶剂化环境,有利于TFSI阴离子的参与,从而促进了富含LiF和Li₃N的坚固固体电解质界面(SEI)的形成。结果表明,GPE具有较宽的电化学稳定性窗口(5.3 V vs. Li+/Li),并在0.1 mA cm-2下稳定镀锂/剥离1000小时。此外,LiFePO₄/GPE/Li电池在0.5C下循环500次后的容量保留率为94.9%,而NCM811/GPE/Li电池在150次循环后的放电容量为153.8 mAh g-1,保留率为86.5%。这项工作为高性能锂金属电池的发展建立了一个可扩展和有前途的战略。
{"title":"Interface-stabilized gel polymer electrolyte for high-performance lithium metal batteries","authors":"Chenxi Zhu ,&nbsp;Yan Zhao ,&nbsp;Rui Xu ,&nbsp;Wenqing Lv ,&nbsp;Yao Zhao ,&nbsp;Bin Huang ,&nbsp;Hua-Feng Fei ,&nbsp;Zhijie Zhang","doi":"10.1016/j.jcis.2026.140029","DOIUrl":"10.1016/j.jcis.2026.140029","url":null,"abstract":"<div><div>Lithium metal batteries demand electrolytes that combine high ionic conductivity with mechanical robustness and interfacial stability. This study presents a novel composite gel polymer electrolyte (GPE) engineered by integrating a cyano-functionalized polysiloxane (PCMS) frameworks, diethylene glycol dimethyl ether (DEGDME) plasticizers, and electrospun polyacrylonitrile (PAN) nanofiber scaffolds. The optimized GPE system achieves an exceptional combination of properties: high ionic conductivity (3.3 × 10<sup>−3</sup> S cm<sup>−1</sup> at 30 °C), outstanding Li<sup>+</sup> transference number (0.79), and remarkable mechanical strength (3.9 MPa). Theoretical calculations and experimental analyses collectively confirm that the -CN groups competitively coordinate with Li<sup>+</sup>, restructuring the solvation environment to favor TFSI<sup>−</sup> anion participation, thereby facilitating the formation of a robust solid electrolyte interphase (SEI) enriched with LiF and Li₃N. As a result, the GPE demonstrates a wide electrochemical stability window (5.3 V vs. Li<sup>+</sup>/Li) and stable lithium plating/stripping for 1000 h at 0.1 mA cm<sup>−2</sup>. Additionally, LiFePO₄/GPE/Li full cells achieve 94.9% capacity retention after 500 cycles at 0.5C, while NCM811/GPE/Li cells deliver a high discharge capacity of 153.8 mAh g<sup>−1</sup> with 86.5% retention after 150 cycles. This work establishes a scalable and promising strategy for the development of high-performance lithium metal batteries.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"710 ","pages":"Article 140029"},"PeriodicalIF":9.7,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146130785","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ferroptosis-sensitizing nanoprodrug system for synergistic therapy of triple-negative breast cancer 协同治疗三阴性乳腺癌的致敏纳米前药系统。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-02-03 DOI: 10.1016/j.jcis.2026.140048
Yong Huang , Tao Quan , Bowen Li , Chaohui Zhen , Haiqian Zhang , Zhiyao Li , Chongzhi Wu , Rui Liang , Lihe Sun , Xin Xie
Triple-negative breast cancer (TNBC), lacking effective therapeutic targets, is highly aggressive, prone to metastasis, and associated with poor prognosis, highlighting the necessity for innovative therapeutic strategies. Ferroptosis, an emerging form of iron-dependent programmed cell death, presents a promising treatment approach. However, its effectiveness is often hindered by adaptive resistance within the tumor microenvironment and inefficient drug delivery. To address these limitations, the glutathione (GSH)-responsive disulfide linker (-SS-) was utilized to engineer rhein (Rhe, chemotherapeutic agent) and ferrocene (Fc, ferroptosis booster) into the self-assembling small-molecule prodrug RSSF. Sorafenib (SOR), a ferroptosis inducer, was stably loaded into RSSF via a simple nanoprecipitation method, yielding the newly nanoprodrug designated as SOR@RSSF nanoparticles (NPs) for the combination therapy of TNBC. SOR@RSSF NPs exhibit markedly enhanced cellular uptake and enable the highly specific and synchronous release of Rhe, Fc, and SOR in response to intracellular GSH levels. Notably, Fc efficiently generates hydroxyl radicals (•OH) through the Fenton reaction, thereby inducing pronounced oxidative stress, while SOR concurrently impaired the cellular ferroptosis defense machinery. Combined with the chemotherapeutic activity of Rhe, the resulting lipid peroxide (LPO) accumulation and GSH depletion synergistically trigger both ferroptosis and apoptosis selectively in tumor cells. In a 4T1 tumor-bearing mouse model, SOR@RSSF NPs significantly inhibited tumor progression while maintaining a favorable biosafety profile. Overall, this study presents a promising ferroptosis-sensitizing strategy using a nanoprodrug delivery system for combination therapy against TNBC.
三阴性乳腺癌(triple negative breast cancer, TNBC)侵袭性强,易转移,预后差,缺乏有效的治疗靶点,迫切需要创新的治疗策略。铁下垂是一种新兴形式的铁依赖性程序性细胞死亡,提出了一种有希望的治疗方法。然而,其有效性经常受到肿瘤微环境内适应性耐药和低效给药的阻碍。为了解决这些局限性,利用谷胱甘肽(GSH)响应的二硫连接体(- ss -)将大黄酸(Rhe,化疗药物)和二铁二烯(Fc,铁凋亡增强剂)设计成自组装的小分子前体药物RSSF。Sorafenib (SOR)是一种铁凋亡诱导剂,通过简单的纳米沉淀法稳定地装载到RSSF中,产生新的纳米前体药物SOR@RSSF纳米颗粒(NPs),用于TNBC的联合治疗。SOR@RSSF NPs表现出显著增强的细胞摄取,并使Rhe, Fc和SOR在响应细胞内GSH水平时具有高度特异性和同步释放。值得注意的是,Fc通过芬顿反应有效地产生羟基自由基(•OH),从而诱导明显的氧化应激,而SOR同时损害了细胞的铁凋亡防御机制。结合Rhe的化疗活性,由此产生的脂质过氧化(LPO)积累和GSH消耗协同触发肿瘤细胞的铁下垂和选择性凋亡。在4T1荷瘤小鼠模型中,SOR@RSSF NPs显著抑制肿瘤进展,同时保持良好的生物安全性。总的来说,这项研究提出了一种有前途的铁致敏策略,使用纳米前药物递送系统联合治疗TNBC。
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引用次数: 0
Synergistic space-electron regulation under interlayer confinement: Disrupting oxygen evolution/reduction reaction scaling relations via dual-pathway control 层间约束下的协同空间电子调控:通过双途径控制破坏析氧/还原反应缩放关系。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-01-30 DOI: 10.1016/j.jcis.2026.140016
Xinyi Lu , Haicai Huang , Yihui Bao , Yanyan Xia , Zhencheng Ye , Houyang Chen
Oxygen evolution and reduction reactions (OER/ORR) are fundamental to energy conversion technologies such as water electrolyzers and fuel cells. However, the intrinsic linear scaling relationship (LSR) between the intermediate adsorption energies limits catalytic activity. Overcoming this limitation could surpass the conventional activity-volcano relationship and unlock high-performance OER/ORR electrocatalysts. Herein, we propose a novel interlayer-confinement engineering strategy, utilizing spatially confined dual active sites in interlayer-confined dual single-atom-catalysts (iDSACs), to fundamentally break the intrinsic LSR by simultaneously manipulating reaction pathways and intermediate adsorption. Density functional theory (DFT) computations demonstrate that the synergistic space-electron effects enhance charge transfer, activate the O–O bond, and facilitate its dissociation. Further, tuning the confinement strength exerts opposing effects on various intermediates and catalysts. Consequently, this strategy effectively disrupts the LSR between *OOH and *OH adsorption, thereby improving OER and ORR activities. Additionally, an optimal interlayer distance of 7.0 Å is identified to balance dual-site synergy and steric effects, achieving low overpotentials (0.26 V for OER and 0.30 V for ORR on IrN4). This work establishes space-electron synergy as a generic platform to disrupt adsorption scaling laws, advancing efficient electrocatalyst design and providing fundamental insights into confined electrocatalysis.
氧释放和还原反应(OER/ORR)是能量转换技术的基础,如水电解槽和燃料电池。然而,中间吸附能之间固有的线性标度关系限制了催化活性。克服这一限制可以超越传统的活火山关系,并开发出高性能的OER/ORR电催化剂。在此,我们提出了一种新的层间约束工程策略,利用层间约束双单原子催化剂(iDSACs)中的空间限制双活性位点,通过同时操纵反应途径和中间吸附,从根本上打破本征LSR。密度泛函理论(DFT)计算表明,协同空间电子效应增强了电荷转移,激活了O-O键,并促进了O-O键的解离。此外,调节约束强度对各种中间体和催化剂产生相反的影响。因此,该策略有效地破坏了*OOH和*OH吸附之间的LSR,从而提高了OER和ORR活性。此外,确定了7.0 Å的最佳层间距离,以平衡双位点协同作用和位阻效应,实现低过电位(IrN4上OER为0.26 V, ORR为0.30 V)。这项工作建立了空间电子协同作用作为破坏吸附结垢规律的通用平台,推进了高效的电催化剂设计,并为受限电催化提供了基本见解。
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引用次数: 0
K+ pre-intercalation tailored interlayer hydration engineering in hydrated V2O5: A high-capacity and ultrastable cathode for aqueous zinc-ion batteries 水合V2O5中K+预插层定制层间水化工程:一种高容量超稳定锌离子电池阴极材料。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-02-02 DOI: 10.1016/j.jcis.2026.140037
Tiezhong Liu, Huazhen Fei, Canwei Zheng, Pengjin Li, Zhiwei Xia, Can Huang, Shuang Hou, Qiang Deng, Tingting Liu, Lingzhi Zhao
Hydrated V2O5 is a promising cathode material for aqueous zinc-ion batteries (ZIBs), where interlayer structural H2O plays a crucial role in tuning Zn2+ storage performance. Nevertheless, the precise modulation of interlayer H2O content remains a major challenge in material synthesis. Herein, we employ pre-intercalated K+ ions as structural mediators to modulate the interlayer H2O content in hydrated V2O5, successfully synthesizing K0.4V2O5·0.24H2O (KVOH) with an optimized hydrated structure. The engineered hydration structure creates a greatly favorable interlayer electrostatic shielding microenvironment that effectively weakens the attraction between intercalated Zn2+ and VO framework, thereby facilitating highly reversible and rapid Zn2+ (de)intercalation. Simultaneously, the pre-intercalated K+ ions and interlayer H2O molecules act as structural pillars that cooperatively stabilize the host framework during prolonged charge/discharge cycling. Benefiting from these advantages, KVOH delivers a high zinc storage capacity of 469.6 mAh g−1 at 0.5 A g−1 and maintains 88.2% of its initial capacity after 500 cycles. Moreover, it also demonstrates outstanding long-term cycling stability, achieving 79.0% capacity retention after 5000 cycles at 10 A g−1. This work reveals the crucial role of interlayer hydration chemistry in governing Zn2+ storage performance and provides a novel strategy for precisely modulating interlayer water content in hydrated V2O5 cathodes.
水合V2O5是一种很有前途的水性锌离子电池正极材料,其层间结构的H2O对Zn2+的存储性能起着至关重要的调节作用。然而,层间水含量的精确调制仍然是材料合成中的一个主要挑战。本文采用预插层K+离子作为结构介质调节水合V2O5中层间H2O含量,成功合成了水合结构优化的K0.4V2O5·0.24H2O (KVOH)。工程水化结构创造了一个非常有利的层间静电屏蔽微环境,有效地减弱了嵌入Zn2+和VO框架之间的吸引力,从而促进了Zn2+的高可逆和快速嵌入。同时,预插入的K+离子和层间的H2O分子作为结构支柱,在长时间的充放电循环中协同稳定宿主框架。得益于这些优势,KVOH在0.5 a g-1下可提供469.6 mAh g-1的高锌存储容量,并在500次循环后保持其初始容量的88.2%。此外,它还表现出出色的长期循环稳定性,在10 A g-1下循环5000次后,容量保持率达到79.0%。这项工作揭示了层间水化化学在控制Zn2+存储性能中的关键作用,并为精确调节水合V2O5阴极层间含水量提供了一种新的策略。
{"title":"K+ pre-intercalation tailored interlayer hydration engineering in hydrated V2O5: A high-capacity and ultrastable cathode for aqueous zinc-ion batteries","authors":"Tiezhong Liu,&nbsp;Huazhen Fei,&nbsp;Canwei Zheng,&nbsp;Pengjin Li,&nbsp;Zhiwei Xia,&nbsp;Can Huang,&nbsp;Shuang Hou,&nbsp;Qiang Deng,&nbsp;Tingting Liu,&nbsp;Lingzhi Zhao","doi":"10.1016/j.jcis.2026.140037","DOIUrl":"10.1016/j.jcis.2026.140037","url":null,"abstract":"<div><div>Hydrated V<sub>2</sub>O<sub>5</sub> is a promising cathode material for aqueous zinc-ion batteries (ZIBs), where interlayer structural H<sub>2</sub>O plays a crucial role in tuning Zn<sup>2+</sup> storage performance. Nevertheless, the precise modulation of interlayer H<sub>2</sub>O content remains a major challenge in material synthesis. Herein, we employ pre-intercalated K<sup>+</sup> ions as structural mediators to modulate the interlayer H<sub>2</sub>O content in hydrated V<sub>2</sub>O<sub>5</sub>, successfully synthesizing K<sub>0.4</sub>V<sub>2</sub>O<sub>5</sub>·0.24H<sub>2</sub>O (KVOH) with an optimized hydrated structure. The engineered hydration structure creates a greatly favorable interlayer electrostatic shielding microenvironment that effectively weakens the attraction between intercalated Zn<sup>2+</sup> and V<img>O framework, thereby facilitating highly reversible and rapid Zn<sup>2+</sup> (de)intercalation. Simultaneously, the pre-intercalated K<sup>+</sup> ions and interlayer H<sub>2</sub>O molecules act as structural pillars that cooperatively stabilize the host framework during prolonged charge/discharge cycling. Benefiting from these advantages, KVOH delivers a high zinc storage capacity of 469.6 mAh g<sup>−1</sup> at 0.5 A g<sup>−1</sup> and maintains 88.2% of its initial capacity after 500 cycles. Moreover, it also demonstrates outstanding long-term cycling stability, achieving 79.0% capacity retention after 5000 cycles at 10 A g<sup>−1</sup>. This work reveals the crucial role of interlayer hydration chemistry in governing Zn<sup>2+</sup> storage performance and provides a novel strategy for precisely modulating interlayer water content in hydrated V<sub>2</sub>O<sub>5</sub> cathodes.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"710 ","pages":"Article 140037"},"PeriodicalIF":9.7,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146130698","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Realizing high-performance wood-based piezoresistive sensing through an interfacial bridging approach for wearable functional integration 基于可穿戴功能集成的接口桥接方法实现高性能木基压阻传感。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-02-04 DOI: 10.1016/j.jcis.2026.140052
Hao Shen , Junlan Gao , Min Yu , Shengquan Liu , Fuquan Xiong
Wood-based aerogels have garnered widespread attention in flexible wearable electronics owing to their sustainability, low density, and high porosity. However, extant wood-based aerogel sensors often struggle to balance high sensitivity, broad detection range, and long-term stability, primarily due to the irregular conductive filler dispersion and weak interfacial bonding within the cellulose framework. Herein, the covalent-noncovalent interfacial bridging strategy was developed to fabricate a MXene/carbon nanotube (CNT) wood aerogel piezoresistive sensor with a layered porous structure and an abundant, stable 3D conductive network. The aerogel exhibited superior elasticity (96.70% stress retention after 1000 cycles at 50% compression strain), a broad detection range (0–160 kPa), and high sensitivity (13.76 kPa−1), outperforming most reported biomass-based aerogel sensors. This performance enables reliable operation across diverse applications, including physiological monitoring, human motion detection, information encoding, and wireless real-time robot control. Furthermore, when integrated with machine learning, the sensor achieves 99.44% accuracy in recognizing different hand gestures. This study presents an innovative and sustainable design strategy for high-performance wood aerogel sensors aimed at advanced flexible electronic applications.
木基气凝胶由于其可持续性、低密度和高孔隙率而在柔性可穿戴电子产品中引起了广泛的关注。然而,现有的木基气凝胶传感器往往难以平衡高灵敏度、宽检测范围和长期稳定性,这主要是由于纤维素框架内导电填料分散不规则和界面结合弱。本文采用共价-非共价界面桥接策略,制备了具有层状多孔结构和丰富、稳定的三维导电网络的MXene/碳纳米管(CNT)木气凝胶压阻传感器。该气凝胶具有优异的弹性(在50%压缩应变下1000次循环后应力保持率为96.70%),检测范围宽(0-160 kPa),灵敏度高(13.76 kPa-1),优于大多数报道的生物质气凝胶传感器。这种性能可以在各种应用中实现可靠的操作,包括生理监测,人体运动检测,信息编码和无线实时机器人控制。此外,当与机器学习相结合时,传感器识别不同手势的准确率达到99.44%。本研究提出了一种针对先进柔性电子应用的高性能木材气凝胶传感器的创新和可持续设计策略。
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引用次数: 0
Universal quenching-reduction engineering of controllable Cu0/Cu+ active sites in 2D heterojunctions for enhanced Fenton-like catalysis 二维异质结中可控Cu0/Cu+活性位点的通用淬火还原工程增强类芬顿催化。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-01-28 DOI: 10.1016/j.jcis.2026.139997
Can Peng , Zhengyan Yu , Fengjiao Zhou , Jiajin Lin , Aihua Xu , Xiuying Liu , Shuaiqi Zhao , Xiaoxia Li
The construction of stable Cu0/Cu+ active sites is essential for achieving high-performance copper-based Fenton-like catalysis. In this work, we develop a novel ethanol-mediated quenching reduction strategy synergistically integrated with rational two-dimensional structural engineering to precisely construct and stabilize Cu0/Cu+ pairs within a two-dimensional Cu-CuO/TiO2 heterojunction (CTO-Q). The approach leverages the transient thermal energy generated during rapid cooling to initiate ethanol dehydrogenation, during which in-situ electrons are released and subsequently reduce Cu2+ ions, thereby facilitating the controlled formation and long-term stabilization of coexisting Cu0/Cu+ species. Advanced spectroscopic characterizations provide direct evidence for the successful generation and chemical state stability of the Cu0/Cu+ active sites. The resultant CTO-Q catalyst exhibits superior PMS activation capability, achieving 95% removal of levofloxacin within 30 min, with an observed rate constant (kobs = 0.35 min−1) that is 3.89-fold higher than that of the conventional catalyst. Remarkably, the catalytic performance remains nearly unchanged after five consecutive cycles, maintaining approximately 95% degradation efficiency, which underscores its exceptional operational stability—attributable to a self-sustaining redox cycle that mitigates irreversible oxidation. The generality and scalability of this synthetic strategy are further validated by the successful fabrication of a family of two-dimensional Cu-based heterojunctions (Cu-CuO/CeO2, Cu-CuO/SiO2, and Cu-CuO/Al2O3). Critically, this methodology enables the valorization of Fenton sludge into a high-efficiency catalytic material, thereby establishing a direct link between advanced functional material design and sustainable environmental remediation.
构建稳定的Cu0/Cu+活性位点是实现高性能铜基类芬顿催化的关键。在这项工作中,我们开发了一种新的乙醇介导的淬火还原策略,与合理的二维结构工程协同集成,在二维Cu- cuo /TiO2异质结(CTO-Q)中精确构建和稳定Cu0/Cu+对。该方法利用快速冷却过程中产生的瞬态热能引发乙醇脱氢,在此过程中,原位电子被释放,随后Cu2+离子被还原,从而促进Cu0/Cu+共存物质的可控形成和长期稳定。先进的光谱表征为Cu0/Cu+活性位点的成功生成和化学状态稳定性提供了直接证据。合成的CTO-Q催化剂表现出优异的PMS活化能力,在30 min内达到95%的左氧氟沙星去除率,观察到的速率常数(kobs = 0.35 min-1)是传统催化剂的3.89倍。值得注意的是,在连续5个循环后,催化性能几乎保持不变,保持约95%的降解效率,这强调了其卓越的运行稳定性,这归因于一个自我维持的氧化还原循环,减轻了不可逆氧化。通过成功制备一系列二维cu基异质结(Cu-CuO/CeO2, Cu-CuO/SiO2和Cu-CuO/Al2O3),进一步验证了该合成策略的通用性和可扩展性。至关重要的是,该方法使Fenton污泥转化为高效的催化材料,从而在先进功能材料设计和可持续环境修复之间建立了直接联系。
{"title":"Universal quenching-reduction engineering of controllable Cu0/Cu+ active sites in 2D heterojunctions for enhanced Fenton-like catalysis","authors":"Can Peng ,&nbsp;Zhengyan Yu ,&nbsp;Fengjiao Zhou ,&nbsp;Jiajin Lin ,&nbsp;Aihua Xu ,&nbsp;Xiuying Liu ,&nbsp;Shuaiqi Zhao ,&nbsp;Xiaoxia Li","doi":"10.1016/j.jcis.2026.139997","DOIUrl":"10.1016/j.jcis.2026.139997","url":null,"abstract":"<div><div>The construction of stable Cu<sup>0</sup>/Cu<sup>+</sup> active sites is essential for achieving high-performance copper-based Fenton-like catalysis. In this work, we develop a novel ethanol-mediated quenching reduction strategy synergistically integrated with rational two-dimensional structural engineering to precisely construct and stabilize Cu<sup>0</sup>/Cu<sup>+</sup> pairs within a two-dimensional Cu-CuO/TiO<sub>2</sub> heterojunction (CTO-Q). The approach leverages the transient thermal energy generated during rapid cooling to initiate ethanol dehydrogenation, during which in-situ electrons are released and subsequently reduce Cu<sup>2+</sup> ions, thereby facilitating the controlled formation and long-term stabilization of coexisting Cu<sup>0</sup>/Cu<sup>+</sup> species. Advanced spectroscopic characterizations provide direct evidence for the successful generation and chemical state stability of the Cu<sup>0</sup>/Cu<sup>+</sup> active sites. The resultant CTO-Q catalyst exhibits superior PMS activation capability, achieving 95% removal of levofloxacin within 30 min, with an observed rate constant (k<sub>obs</sub> = 0.35 min<sup>−1</sup>) that is 3.89-fold higher than that of the conventional catalyst. Remarkably, the catalytic performance remains nearly unchanged after five consecutive cycles, maintaining approximately 95% degradation efficiency, which underscores its exceptional operational stability—attributable to a self-sustaining redox cycle that mitigates irreversible oxidation. The generality and scalability of this synthetic strategy are further validated by the successful fabrication of a family of two-dimensional Cu-based heterojunctions (Cu-CuO/CeO<sub>2</sub>, Cu-CuO/SiO<sub>2</sub>, and Cu-CuO/Al<sub>2</sub>O<sub>3</sub>). Critically, this methodology enables the valorization of Fenton sludge into a high-efficiency catalytic material, thereby establishing a direct link between advanced functional material design and sustainable environmental remediation.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"710 ","pages":"Article 139997"},"PeriodicalIF":9.7,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146099696","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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Journal of Colloid and Interface Science
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